Bridge-rich and loop-less hydrogel networks through suppressed micellization of multiblock polyelectrolytes

Jihoon Han, Saeed Najafi, Youyoung Byun, Lester Geonzon, Seung-Hwan Oh, Jiwon Park, Jun Mo Koo, Jehan Kim, Taehun Chung, Im Kyung Han, Suhun Chae, Dong Woo Cho, Jinah Jang, Unyong Jeong, Glenn H. Fredrickson, Soo-Hyung Choi, Koichi Mayumi, Eunji Lee (), Joan-Emma Shea () and Youn Soo Kim ()
Additional contact information
Jihoon Han: Pohang University of Science and Technology (POSTECH)
Saeed Najafi: University of California
Youyoung Byun: Gwangju Institute of Science and Technology (GIST)
Lester Geonzon: Kashiwa
Seung-Hwan Oh: Hongik University
Jiwon Park: Gwangju Institute of Science and Technology (GIST)
Jun Mo Koo: Chungnam National University
Jehan Kim: Pohang University of Science and Technology (POSTECH)
Taehun Chung: Pohang University of Science and Technology (POSTECH)
Im Kyung Han: Pohang University of Science and Technology (POSTECH)
Suhun Chae: Pohang University of Science and Technology (POSTECH)
Dong Woo Cho: Pohang University of Science and Technology (POSTECH)
Jinah Jang: Pohang University of Science and Technology (POSTECH)
Unyong Jeong: Pohang University of Science and Technology (POSTECH)
Glenn H. Fredrickson: University of California
Soo-Hyung Choi: Hongik University
Koichi Mayumi: Kashiwa
Eunji Lee: Gwangju Institute of Science and Technology (GIST)
Joan-Emma Shea: University of California
Youn Soo Kim: Pohang University of Science and Technology (POSTECH)

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Most triblock copolymer-based physical hydrogels form three-dimensional networks through micellar packing, and formation of polymer loops represents a topological defect that diminishes hydrogel elasticity. This effect can be mitigated by maximizing the fraction of elastically effective bridges in the hydrogel network. Herein, we report hydrogels constructed by complexing oppositely charged multiblock copolymers designed with a sequence pattern that maximizes the entropic and enthalpic penalty of micellization. These copolymers self-assemble into branched and bridge-rich network units (netmers), instead of forming sparsely interlinked micelles. We find that the storage modulus of the netmer-based hydrogel is 11.5 times higher than that of the micelle-based hydrogel. Complementary coarse grained molecular dynamics simulations reveal that in the netmer-based hydrogels, the numbers of charge-complexed nodes and mechanically reinforcing bridges increase substantially relative to micelle-based hydrogels.

Date: 2024
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DOI: 10.1038/s41467-024-50902-z

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